Method of testing thermal neutron fissionable material for purity



Jan. 24, 1961 E. FERMI ETAL 2,969,307 D OF TESTING THERM METHO AI.. NEUT FISSIONA MATER FO URI Fi Nov. 19

FLE-l ffy/ United States NIETHOD OF TESTING THERMAL NEUTRON FISSIONABLE MATERIAL FOR PURITY Filed Nov. 21, 1945, Ser. No. 630,123

1 Claim. (Cl. 204-154.2)

This invention relates toa novel method of testing the neutronic purity of uranium or other material tobe used in a neutronic reactor.

In neutronic reactors a neutron ssionable isotope such as U233, U235, or 94239 or mixtures thereof is subjected to fission by absorption of neutrons, and a self-sustaining chain reaction is established by the neutrons evolved by the fission. In general such reactors comprise bodies of compositions containing such ssionable material, for example, natural uranium, disposed ina material that slows the neutrons to thermal energies. Such a material is termed a neutron moderator. Carbon and D20 (heavy water) are typical moderators suitable for such use.` Heat is evolved during the reaction which is removed by passage of a coolant through the reactor in heat exchange relationship therewith. Specific details of the theory and essential characteristics of such reactors are set forth in copending application of Enrico Fermi and Leo Szilard, Serial No. 568,904, filed Dec. 19, 1944, now Patent 2,708,656, dated May 17, 1955.

-It has been found that certain impurities or neutron absorbers, which do not take part in the reaction involving fission of an isotope and formation vof afssionable isotope, exert a marked depressing action upon the neutron chain reaction. Unless the amount of such absorbers is controlled within proper limits, a self-sustaining reaction cannot be maintained. Where a material such as natural uranium is used to establish the reaction even very `small amounts of certain impurities or absorbers will prevent maintenance of the reaction. Furthermore, they are speciiic to natural uranium and will vary with a change in the iissionable material used in the pile.' It is an object of the inventionto provide a novel methodof determining the neutronic purityof material, such as uranium, to be used in a neutronic reactor. Neutronic purity, as hereinafter more fully discussed, has no necessary connection with.chemical purity, i.e., a composition having high neutronic purity is vone which is substantially free from particular elements having relatively Vgreat neutron capture cross-sections.

An initial number. of fast neutrons in the system, by going through the process of absorption and fission, produce in the next generation a number of neutrons generally different from the initial number. The ratio of the number produced after one generation to the initial number Vfor a system of infinite size is called the reproduction or multiplication factor of the system and is denoted by the symbol K. i

For any nite system, some neutrons will escape from the periphery Vof the system. Consequently a system of finite size may be said to have a K constant, even though the value thereof would only exist if the system as built were extended to infinity without change of geometry or materials. Thus when K is referred to herein as a constant of a system of practical size, it always refers to what would exist in the same type of system of infinite size.A If K can be made suiciently greater than unity to atent ICC indicate a net gain in neutrons in the theoretical system of infinite size, and then an actual system is built to be sufliciently large so that this gain is not entirely lost by leakage from the exterior surface of the system, then a self-sustaining chain reacting system of finite and practical size can be built to produce power and related byproducts by nuclear Iission of natural uranium. The neutron reproduction ratio in a system of finite size, therefore, differs from K by the external leakage factor, and by a factor due to the neutron absorption by localized neutron absorber, and the reproduction ratio must still be sufficiently greater than unity to permit the neutron density to rise exponentially with time in the system as built.' v

During the interchange of neutrons `in a system of finite size, comprising bodies of any size disposed in a neutron moderator, neutrons may be lost to the chain reaction in four ways:

(1) By absorption or capture in the uranium content Vof the bodies without producing fission,

rial itself,

(3) By leakage rout Vof the system throughvthe peripheryv thereof, and' (4) By absorptionror capture by the impurities present in both the uranium'bodies and the moderator. Y

However,even when. the first three above-mentioned losses are reduced to apractical minimum'f'no self-sustaining chain reaction can be obtained eine' any system unless impurities inthe material used forlthetlactoare' reduced to such an extent that the lossbyeparasitic capture by suchrimpuritiesY will not prevent the `reaction ffroni becoming self-sustaining. Impurities presentY ineboth the uranium and the moderator consequently constitute a very important neutron loss factor in `the chain. The effectiveness of various elements as neutronlabsorbers varies tremendously.

Certain elements such as boron, cadmium, samarium, gadolinium, 'and some others, if present even in a few parts per million, could very likely prevent a self-sustain-v ing chain reaction from taking place. It is highly important, therefore, to remove as far as possible all impurities capturing neutrons to the detriment of the chain reaction from both the slowing material and the uranium.' If these impurities are present in too great quantity, the self-sustaining chain reaction cannot be attained. The permissible amounts of impurities will vary for each specific geometry, depending upon such considerations the form in which the uranium is used-that is, whether natural or enriched, whether as metal or oxide. The type of slowing-down material used, for example, whether deuterium, graphite, or beryllium, also influences the effect of impurities, as do the weight ratios between the*y uranium and the slowing-down material. t

The eect of impurities on the optimum reproduction factor K may be conveniently evaluated by means of certain constants known as danger coeflcients which are assigned to the various elements. These danger coefficients for the impurities are leach multiplied by the frac, tion by weight of the corresponding impurity, withre spect to the Weight of uranium in the system; and the total sum of these coefficients gives a value known as the total danger sum. This total danger sum is ysubtracted from the reproduction factor K as calculated for' pure' materials under consideration. Y

The danger coefficients are defined in terms of the ratio of the weight of impurity per unit mass of uranium and are based on the cross-section for absorption of neutrons of the various elements. These values may be obtained` from published literature on the subject such asv yPhy 3 schrift fr Physik, vol. 121, p. 201 (1943), and the danger coecient computed by the formula wherein T, representsI the cross section `for the impurity and Twthe cross .section-.forthe uranium,'A1 theuatomic weight of :the impurity and .Au .the atomic weight for uranium. 1 In.general, whether the impurities are in the moderator` or.in `theuranium, they may be 4computed as theirffractionfby'thef.weight-of the uraniumvin the system andthe :result will*betsucientlyfaccurate for design purposes.

f Theapproximate dangercoecients for some `elements in a natural uranium system are given in the following table, `wherein the elements are `listed in orderof their atomic number:

'I'hesum' of the danger coelcientsv ofthe impurities in vanygiven composition entering into a reactor as multiplied by 'the' fraction by weight of the uranium in the reactor 'is known 'as total danger sum of the composition. This gure Vis a dimensionless constant like K and accordingly can be directly subtracted from K. It will be noted that vthe danger coefcients given are related to the neutron danger coefficient of unity for uranium.

`As a*spe`cific example, if the materials of a system under' considerationhave 0.01 percent by weight of each ofthe elements' N, Co, and Ag with respect to the weight ofv the uranium in the system, the total danger sum in K units for such an analysis would be:

A'Ihis figure' can -then be subtracted from the'K calculatedor theoretically pure materials to Ygive the actual K :factor for the `geometry and material used. This would be la rather unimportant reduction in thereproduction V"ract'orLK unless thereproduction factor VK for-a given geometry and materials without considering impurities, isvery nearly-unity. If, on the other hand, the impurities in the uranium are Li, Co, aud Agin the same percentage, theftotahdanger sum would be:

.0310+.00l7+.0018=.0345 `reduction linA K'duefto impurities.

"fThejmaXimum `possible K factors for `natural-uranium ueutronic 'reaction systems 'when optimum geometry is 4 used and where the materials used are assumed to be theoretically pure, have been calculated as follows:

It can` be readilyiseen-from the above tabulation that the total danger sum for impurities in boththeuranium and moderatormust beless :than .3 in order that the K factor remain equal to or `greater than unity with a moderator having a minimumV absorption of neutrons, a deuterium moderator, less than .09 for a beryllium oxide moderator, and less than .1 for a graphite moderator. Even when neutron losses due to moderator and leakage have been substantially eliminated, the danger sum of the impurities or absorbers in the"natura1`uranium can not exceed about 0.3.

The present invention comprehends a verypractical method oftestingmateriahsuch `as uranium, said method being known 'as the "shot`gun'te`st. In this testa thin neutron detector, e.g., a piece of `indium foil, placed near a neutron source inside a block of parafn is made radioactive by an amount proportionaltothe density of thermal neutrons atthe foil and the time'of exposure. This radioactivity can'beV measured. `A neutron absorbing pellet 'suchlas one' of a standard-'amount of boron, when placed close to the detectorfoiL'decreases the thermal-neutron density inthe neighborhood ofthe foil and lowers the induced radioactivity of the detector foil. By replacing the standard boron absorbing pellet with a pellet containing theimpurities from a known amount ofuranium composition to betested, and again measuring the radioactivityof the neutron detector, a direct comparison `is obtained `between the absorption caused by the unknown composition and the standard boron absorber. From this comparison the danger sum of the impurities in the uranium composition can be calculated in terms of boron equivalent. From the danger coeflicient of boron the K reduction can becalculated.

y OneV suitable means forcarrying out the shotgun testis described below, although fsuch' meansisnot' part of the' present invention. -It is' also illustrated in the accompanying drawing, wherein Figure l'is a cross-sectional View of `the apparatus `during measurement of the `radioactivity on `an indium foil without a pellet; Figure 2is a topview of the lower box along line Z-Ziof `Figure l; Figure 3 isan .enlarged view of the apparatus along A"line 3--3 of Figure 1 after insertion of the pellet of uranium impurities; and Figure 4fisacross`sectional`view ofthe apparatus like that of Figure 3 after insentionfof astandard boronpellet.

A block.10iof paratlin 30cm.` on eachlside is moldedin a wooden box 11. vThe box:andthe` parain box-are cut in halves 12, 13 and 14, 15, respectively, horizontally sothat `each half of the. parafn remains in itsown-portion of the box. A hole 16.5is formed throughi one `iside ofthe upper box half `and into the. paratin` 3fcm. above and parallel-to :the lowersurfaceof theiparatnyfthis hole 16 extends into the center of theparafiin. JThe adjacent paran surfaces of'ltheablo'ck :halves `arercoveredy the upper with onion skin paper 17, thelowerwithf'celloplane 18 .linked at theibackvwith Scotch .tapel 19.1,(Fig'ure 2) to permit liftingfor access to the paran surface. `The upper half of fthe box is supported so that itcanbe readily moved up anddown, and the lower half `of the-box is supported so that vit can slide in and outzlike adrawer when the upper half is up. A-.small square hole: 20 is cut inthe center of the-upper surface of the lower` block of paraffin a little more than''g of an inchldeep.

Itis knownthat 3 cm. ofparatlin will slow down the neutrons evolved from a radium-beryllium source to slow n l. A

or thermal speeds. A radium-beryllium source 20a consisting of 200.5 mg. of radium and 0.6 gm. of beryllium emitting about 2 l06 neutrons per second may be used as the source. This source is contained in a brass capsule 20b at the end of a long handle 20c.

In order to make a measurement, the composition to be measured is formed into a pellet 21 of predetermined size and shape by hydraulic pressure. This pellet 21 is placedv in an aluminum container 22 which just fits the square hole 20 in the upper surface of the lower half 15 of the parain block 13 and a piece of indium foil 23 is placed carefully over the aluminum container 22 on the surface of the lower paraihn block 13. The lower block 13 is then put in place and the upper block 12 is lowered on top of it. The radium-beryllium source 20a is then inserted all the way into the hole 16 in the upper block, `and exact notations are made of the time. The irradiation is allowed to continue for a set time, usually 15 minutes. It is important that the time be measured accurately and preferably should be the same for all comparable tests.

Preferably, exactly 15 minutes after starting the irradiation, the source is removed. The upper parain block 12 is lifted, the lower paraihn block 13 is slid out, and the indium foil 23 is removed. The foil is then wrapped around the tube of a Geiger-Mller counter (not shown), and preferably exactly 3 minutes after the end of the irradiation counting is begun and continued for exactly 21 minutes.

The counting is preferably started exactly 3 minutes after the end of the irradiation in order to allow the short-lived radiation of the indium, which has a half-life of 13 seconds, to substantially disappear, although mathematical correction can be made, if the time element of either irradiation or counting is charted.

It is important that every precaution be taken to avoid contamination of the foil 23 or Geiger-Mller counter with UX or other foreign substances. Every precaution must be taken to obtain strict cleanliness and to repeat each test in exactly the same way, so as to make all measurements comparable. The details of technique necessary to obtain these results will be obvious to those skilled in the art.

In order to use the shotgun test so as to determine the neutronic purity of uranium to be used in a neutronic reactor, a practical procedure is to take a representative sample of material having a kg. uranium content after large-scale purification as by the methods disclosed in the parent case. The sample is submitted to an additional extremely exhaustive purification on a laboratory scale. In this way, practically all of the impurities left in the uranium composition to be tested can be removed and the impurities are removed, recovered, and formed into pellet 21 (Figure 3). The sample pellet is then compared with the absorption of the standard boron pellet 24 (Figure 4) in the apparatus described.

The results of the shotgun test are usually reported as percent absorption which is equal to Absorption of impurities expressed in equivalent milligrams of boron Absorption of 10 kilograms of uranium expressed in equivalent milligrams of boron Y In a neutronic reactor:

f=thermal utilization, or the fraction of neutrons absorbed in the uranium.

P=probability of a fast neutron escaping resonance capture. Y Y

E=No. of fast neutrons produced by fast fission per fast neutron produced by thermal fission.

n=No. of fast neutrons produced by thermal fission per thermal neutron absorbed.

where A indicates a small increment in the associated term.

mmm-f2 K f1 where neutrons absorbed in uranium neutrons absorbed in U and moderator neutrons absorbed in uranium neutrons absorbed in U, moderator and impurities NiGai NoGao-i Ni-Gai Fractional absorption (shotgun test) l Y absorption of impurities n.v.NGai

absorption of uranium nvNaGao where n=No. of neutrons per cc. v=velocity (cm./5 sec.)

As a close approximation, the absorption in the moderator and in impurities may be ignored as compared to the absorption in the uranium, i.e., NmGam and NiGa, may be considered negligible.

Fractional absorption= Then & N iGa/i K NGa0 But N iGCL Fractional absorption (shotgun test) NoGao Therefore, as a close approximation, fractional absorption from shotgun test=AK, provided K is approximately unity.

While the theory of nuclear reactions set forth herein is based on the lbest .presently lrn'ovvirerp'erime'ntalfevi-v i dence, the invention is inot limited thereto, ias additionaly experimental datalater discovered may modify the theory'l disclosed,

c Obviously, man3/"modifications may"be"made'inthe A5:

, specific ,embodimentsl disclosed With'c'mt departing from the 'intendedscope of the inventionv v vWliatis, claimed is:

, A metnodoftesting:the.neutronicpurityofa therrrial neutron llssionalnlemateriall sample comprising tlieisteps of producing a; neutronux' eld,vinserting alst'and'ard neutron absorber of knownf'eharacteristics"andfamount.

v in said leld, extractingsubstantially all -of the chemical l .impurities from said sample, replacing saidv standard ab- `sorbei with'all of the impurities from krthe sample of the -ssionable material, `and producing successive indications of the .neutron intens-ityby bombardmentI of a neutron f detectorv foil placed at aregion-of said ieldl with both the f absorberand die= impurity sample removed,r with the alif sorber present and theimpuri-tysarnple removed, and with the yabsorber removed yand the impurity ysample present,

whereby the neutronc purity of ,the .sample'm'ay be oak culated from said indications.v f f f v f f l 1 lReferences Cited` in thedile of this patent UNHED"STIFES PATENTS' f v l OTHER kniniERENCES Burgeret al.: zfDetermination of .HydrogenContent by rSlow-Neutron Scattering, ABCD-2319, 3U.S,A.E.:C., 9 v f pagesdate of manuscript, October .21. 1943; date `declassified, September 22, 1.1948.. '(CopylixrPatentQOlce PhyzRev. 55, 5l 1-51?.y (51939). y(Copyin PatentOce f Library.) 

